► At present, the energy of a single isolated attosecond pulse is limited to nanojoule levels. As a result, an intense femtosecond pulse has always…
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▼ At present, the energy of a single isolated attosecond pulse is limited to nanojoule levels. As a result, an intense femtosecond pulse has always been used in combination with a weak attosecond pulse in time-resolved experiments. To reach the goal of conducting true attosecond pump-attosecond probe experiments, a high flux laser source has been developed that can potentially deliver microjoule level isolated attosecond pulses in the 50 eV range, and a unique experimental end station has been fabricated and implemented that can provide precision control of the attosecond-attosecond pump-probe pulses. In order to scale up the attosecond flux, a unique Ti:-Sapphire laser system with a three-stage amplifier that delivers pulses with a 2 J energy at a 10 Hz repetition rate was designed and built. The broadband pulse spectrum covering from 700 nm to 900 nm was generated, supporting a pulse duration of 12 fs. The high flux high-order harmonics were generated in a gas tube filled with argon by a loosely focused geometry under a phase-matching condition. The wavefront distortions for the driving laser were corrected by a deformable mirror with a Shack-Hartmann sensor to significantly improve the extreme ultraviolet radiation conversion efficiency due to the excellent beam profile at focus. A high-damage-threshold beam splitter is demonstrated to eliminate energetic driving laser pulses from high-order harmonics. The extreme ultraviolet pulse energy is measured to be 0.3 microjoule at the exit of the argon gas target. The experimental facilities developed will lead to the generation of microjoule level isolated attosecond pulses and the demonstration of true atto pump-atto probe experiments in near future. Finally, in experiment, we show the first demonstration of carrier-envelope phase controlled filamentation in air using millijoule-level few-cycle mid-infrared laser pulses.
Advisors/Committee Members: Chang, Zenghu.

► Dynamics occurring on microscopic scales, such as electronic motion inside atoms and molecules, are governed by quantum mechanics. However, the Schroedinger equation is usually too…
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▼ Dynamics occurring on microscopic scales, such as electronic motion inside atoms and molecules, are governed by quantum mechanics. However, the Schroedinger equation is usually too complicated to solve analytically for systems other than the hydrogen atom. Even for some simple atoms such as helium, it still takes months to do a full numerical analysis. Therefore, practical problems are often solved only after simplification. The results are then compared with the experimental outcome in both the spectral and temporal domain. For accurate experimental comparison, temporal resolution on the attosecond scale is required. This had not been achieved until the first demonstration of the single attosecond pulse in 2001. After this breakthrough, "attophysics" immediately became a hot field in the physics and optics community. While the attosecond pulse has served as an irreplaceable tool in many fundamental research studies of ultrafast dynamics, the pulse generation process itself is an interesting topic in the ultrafast field. When an intense femtosecond laser is tightly focused on a gaseous target, electrons inside the neutral atoms are ripped away through tunneling ionization. Under certain circumstances, the electrons are able to reunite with the parent ions and release photon bursts lasting only tens to hundreds of attoseconds. This process repeats itself every half cycle of the driving pulse, generating a train of single attosecond pulses which lasts longer than one femtosecond. To achieve true temporal resolution on the attosecond time scale, single isolated attosecond pulses are required, meaning only one attosecond pulse can be produced per driving pulse. Up to now, there are only a few methods which have been demonstrated experimentally to generate isolated attosecond pulses. Pioneering work generated single attosecond pulse using a carrier-envelope phase-stabilized 3.3 fs laser pulse, which is out of reach for most research groups. An alternative method termed as polarization gating generated single attosecond pulses with 5 fs driving pulses, which is still difficult to achieve experimentally. Most recently, a new technique termed as Double Optical Gating (DOG) was developed in our group to allow the generation of single attosecond pulse with longer driving pulse durations. For example, isolated 150 as pulses were demonstrated with a 25 fs driving laser directly from a commercially-available Ti:Sapphire amplifier. Isolated attosecond pulses as short as 107 as have been demonstrated with the DOG scheme before this work. Here, we employ this method to shorten the pulse duration even further, demonstrating world-record isolated 67 as pulses. Optical pulses with attosecond duration are the shortest controllable process up to now and are much faster than the electron response times in any electronic devices. In consequence, it is also a challenge to characterize attosecond pulses experimentally, especially when they feature a broadband spectrum. Similar challenges have previously been met in characterizing…
Advisors/Committee Members: Chang, Zenghu.

► This thesis outlines the high intensity tabletop attosecond extreme ultraviolet laser source at the Institute for the Frontier of Attosecond Science and Technology Laboratory. First,…
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▼ This thesis outlines the high intensity tabletop attosecond extreme ultraviolet laser source at the Institute for the Frontier of Attosecond Science and Technology Laboratory. First, a unique Ti:Sapphire chirped pulse amplifier laser system that delivers 14 fs pulses with 300 mJ energy at a 10 Hz repetition rate was designed and built. The broadband spectrum extending from 700 nm to 900 nm was obtained by seeding a two stage Ti:Sapphire chirped pulse power amplifier with mJ-level white light pulses from a gas filled hollow core fiber. It is the highest energy level ever achieved by a broadband pulse in a chirped pulse amplifier up to the current date. Second, using this laser as a driving laser source, the generalized double optical gating method is employed to generate isolated attosecond pulses. Detailed gate width analysis of the ellipticity dependent pulse were performed. Calculation of electron light interaction dynamics on the atomic level was carried out to demonstrate the mechanism of isolated pulse generation. Third, a complete diagnostic apparatus was built to extract and analyze the generated attosecond pulse in spectral domain. The result confirms that an extreme ultraviolet super continuum supporting 230 as isolated attosecond pulses at 35 eV was generated using the generalized double optical gating technique. The extreme ultraviolet pulse energy was ∼100 nJ at the exit of the argon gas target.
Advisors/Committee Members: Chang, Zenghu.

► Tracking and controlling the dynamic evolution of matter under the influence of external fields is among the most fundamental goals of physics. In the microcosm,…
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▼ Tracking and controlling the dynamic evolution of matter under the influence of external fields is among the most fundamental goals of physics. In the microcosm, the motion of electrons follows the laws of quantum mechanics and evolves on the timescale set by the atomic unit of time, 24 attoseconds. While only a few time-dependent quantum mechanical systems can be solved theoretically, recent advances in the generation, characterization, and application of isolated attosecond pulses and few-cycle femtosecond lasers have given experimentalists the necessary tools for dynamic measurements on these systems. However, pioneering studies in attosecond science have so far been limited to the measurement of free electron dynamics, which can in most cases be described approximately using classical mechanics. Novel tools and techniques for studying bound states of matter are therefore desired to test the available theoretical models and to enrich our understanding of the quantum world on as-yet unprecedented timescales. In this work, attosecond transient absorption spectroscopy with ultrabroadband attosecond pulses is presented as a technique for direct measurement of electron dynamics in quantum systems, demonstrating for the first time that the attosecond transient absorption technique allows for state-resolved and simultaneous measurement of bound and continuum state dynamics. The helium atom is the primary target of the presented studies, owing to its accessibility to theoretical modeling with both ab initio simulations and to model systems with reduced dimensionality. In these studies, ultrafast dynamics – on timescales shorter than the laser cycle – are observed in prototypical quantum mechanical processes such as the AC Stark and ponderomotive energy level shifts, Rabi oscillations and electromagnetically-induced absorption iv and transparency, and two-color multi-photon absorption to “dark” states of the atom. These features are observed in both bound states and quasi-bound autoionizing states of the atom. Furthermore, dynamic interference oscillations, corresponding to quantum path interferences involving bound and free electronic states of the atom, are observed for the first time in an optical measurement. These first experiments demonstrate the applicability of attosecond transient absorption spectroscopy with ultrabroadband attosecond pulses to the study and control of electron dynamics in quantum mechanical systems with high fidelity and state selectivity. The technique is therefore ideally suited for the study of charge transfer and collective electron motion in more complex systems. The transient absorption studies on atomic bound states require ultrabroadband attosecond pulses − attosecond pulses with large spectral bandwidth compared to their central frequency. This is due to the fact that the bound states in which we are interested lie only 15-25 eV above the ground state, so the central frequency of the pulse should lie in this range. On the other hand, the bandwidth needed to generate an isolated 100 as…
Advisors/Committee Members: Chang, Zenghu.

► The goal of this thesis is to design a tabletop coherent soft X-ray source for attosecond high resolution imaging. We collect signals from gas cells…
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▼ The goal of this thesis is to design a tabletop coherent soft X-ray source for attosecond high resolution imaging. We collect signals from gas cells with different length and lens with different focal length. A spectrometer with a grating and a CCD camera is applied to observe and measure the spectrum of the X-ray attosecond pulses.
This thesis first introduces the theory background of ultrafast lasers, then mainly explains high harmonic generation, which is the key method for attosecond pulses generation, subsequently presents the experiment system and analyzes the results from the experiment, also compares different combinations of parameters of the devices.
Advisors/Committee Members: Chang, Zenghu.

► One of the most fundamental goals of attosecond science is to observe and to control the dynamic evolutions of electrons in matter. The attosecond…
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▼ One of the most fundamental goals of attosecond science is to observe and to control the dynamic evolutions of electrons in matter. The attosecond transient absorption spectroscopy is a powerful tool to utilize attosecond pulse to measure electron dynamics in quantum systems directly. In this work, isolated single attosecond pulses are used to probe electron dynamics in atoms and to study dynamics in hydrogen molecules using the attosecond transient absorption spectroscopy technique. The target atom/molecule is first pumped to excited states and then probed by a subsequent attosecond extreme ultraviolet (XUV) pulse or by a near infrared (NIR) laser pulse. By measuring the absorbed attosecond XUV pulse spectrum, the ultrafast electron correlation dynamics can be studied in real time. The quantum processes that can be studied using the attosecond transient absorption spectroscopy include the AC stark shift, multi-photon absorption, intermediate states of atoms, autoionizing states, and transitions of vibrational states in molecules. In all experiments, the absorption changes as a function of the time delay between the attosecond XUV probe pulse and the dressing NIR laser pulse, on a time scale of sub-cycle laser period, which reveals attosecond electron dynamics. These experiments demonstrate that the attosecond transient absorption spectroscopy can be performed to study and control electronic and nuclear dynamics in quantum systems with high temporal and spectral resolution, and it opens door for the study of electron dynamics in large molecules and other more complex systems.
Advisors/Committee Members: Chang, Zenghu.

► The observation of any atomic and molecular dynamics requires a probe that has a timescale comparable to the dynamics itself. Ever since the invention of…
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▼ The observation of any atomic and molecular dynamics requires a probe that has a timescale comparable to the dynamics itself. Ever since the invention of laser, the temporal duration of the laser pulse has been incrementally reduced from several nanoseconds to just attoseconds. Picosecond and femtosecond laser pulses have been widely used to study molecular rotation and vibration.
In 2001, the first single isolated attosecond pulse (1 attosecond = 10^-18 seconds.) was demonstrated. Since this breakthrough, "attoscience" has become a hot topic in ultrafast physics. Attosecond pulses typically have span between EUV to X-ray photon energies and sub-femtosecond pulse duration. It becomes an ideal tool for experimentalists to study ultrafast electron dynamics in atoms, molecules and condensed matter.
The conventional scheme for generating attosecond pulses is focusing an intense femtosecond laser pulse into inert gases. The bound electrons are ionized into continuum through tunneling ionization under the strong electrical field. After ionization, the free electron will be accelerated by the laser field away from the parent ion and then recombined with its parent ion and releases its kinetic energy as a photon burst that lasts for a few hundred attoseconds. According to the classical "three-step model", high order harmonic will have a higher cutoff photon energy when driven by a longer wavelength laser field. Compared to Ti:sapphire lasers center at a wavelength of 800 nm, an optical parametric amplifier could offer a broad bandwidth at infrared range, which could support few cycle pulses for driving high harmonic generation in the X-ray spectrum range.
In this work, an optical parametric chirped-pulse amplification system was developed to deliver CEP-stable 3-mJ, 12-fs pulses centered at 1.7 micron. We implement a chirped-pump technique to phase match the board parametric amplification bandwidth with high conversion efficiency. Using such a laser source, isolated attosecond pulses with photon exceeding 300 eV are achieved by applying the polarization gating technique at 1.7 micron. The intrinsic positive chirp of the attosecond pulses is measured by the attosecond streak camera and retrieved with our PROOF technique. Sn metal filters with negative dispersion were chosen to compensate the intrinsic attochirp. As a result, isolated 53-attosecond soft x-ray pulses are achieved. Such water window attosecond source will be a powerful tool for studying charge distribution/migration in bio-molecules and will bring opportunities to study high field physics or attochemistry.
Advisors/Committee Members: Chang, Zenghu.